Electrolyte Sustaining 4.5 V Li||NCM811 Batteries Cycled at 80°C

doi:10.1002/aenm.70894

Electrolyte Sustaining 4.5 V Li||NCM811 Batteries Cycled at 80°C

2026-04-05

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DOI：10.1002/aenm.70894

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LiNi0.8Mn0.1Co0.1O2 (NCM811)-based lithium metal batteries (LMBs) are widely regarded as promising candidates for next-generation high-energy-density systems. However, under high-temperature and high-voltage conditions, severe interfacial side reactions between the electrolyte and electrodes are inevitably triggered, substantially impeding the practical development of LMBs. Herein, a mechanically and thermally robust LiF/LiBxOy-rich CEI on NCM811 via synergistic regulation of a LiBF4/LiDFOB dual-salt electrolyte and a functional boron-containing additive 2,4,6-tris(3,4,5-trifluorophenyl)boroxin (TTFPB) is rationally constructed. The LiBF4/LiDFOB dual-salt system enhances electrolyte thermal and oxidative stability, while TTFPB reconstructs the Li+ solvation structure by selectively excluding DFOB− from the primary solvation sheath and enriching BF4− coordination, thereby inducing an anion-rich solvation structure. Meanwhile, TTFPB/DFOB− species preferentially decompose at the cathode interphase, generating a uniform and mechanically robust LiF/LiBxOy-rich CEI. This stabilized interphase effectively suppresses continuous electrolyte decomposition and mitigates transition-metals ions (TMs) dissolution, also alleviates cathode phase transitions. Consequently, Li||NCM811 batteries with this electrolyte deliver 80.70% capacity retention after 350 cycles at 4.5 V. Notably, even under extreme operating conditions at 4.5 V and 80°C, the batteries retain 87.50% of their initial capacity after 100 cycles.

Keywords:

cathode electrolyte interphase

high-temperature

high-voltage

lithium metal batteries

Electrolyte Sustaining 4.5 V Li||NCM811 Batteries Cycled at 80°C

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